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Metal-to-insulator crossover in alkali doped zeolite.

ABSTRACT: We report a systematic nuclear magnetic resonance investigation of the (23)Na spin-lattice relaxation rate, 1/T1, in sodium loaded low-silica X (LSX) zeolite, Nan/Na12-LSX, for various loading levels of sodium atoms n across the metal-to-insulator crossover. For high loading levels of n ≥ 14.2, 1/T1T shows nearly temperature-independent behaviour between 10 K and 25 K consistent with the Korringa relaxation mechanism and the metallic ground state. As the loading levels decrease below n ≤ 11.6, the extracted density of states (DOS) at the Fermi level sharply decreases, although a residual DOS at Fermi level is still observed even in the samples that lack the metallic Drude-peak in the optical reflectance. The observed crossover is a result of a complex loading-level dependence of electric potential felt by the electrons confined to zeolite cages, where the electronic correlations and disorder both play an important role.

SUBMITTER: Igarashi M

PROVIDER: S-EPMC4698653 | biostudies-other | 2016

REPOSITORIES: biostudies-other

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Project description:Strategies for designing remarkable nonlinear optical materials using excess electron compounds are well recognized in literature to enhance the applications of these compounds in nonlinear optics. In this study, density functional theory simulations are performed to study alkali and alkaline earth metal-doped benzocryptand using the B3LYP/6-31G+(d, p) level of theory. Vertical ionization energies (VIEs), reactivity parameters, interaction energies, and binding energies exposed the thermodynamic stability of these complexes. FMO analysis revealed that HOMO is located on alkali metals having polarized electrons, which are easy to excite. The doping strategy enhanced the charge transfer with low bandgap energy in the range of 0.68-2.23 eV, which is lower than that of the surface BC (5.50 eV). Also, the lower transition energies and higher oscillator strength indicate that these complexes exhibit excellent electronic and optical properties. Non-covalent interaction analysis suggested the presence of van der Waals interactions between dopants and surface. IR analysis provided information about the frequencies of stretching vibrations present in the complexes due to different bonds. UV-vis analysis revealed that all the newly designed excess electron complexes are transparent in the UV region and possessed maximum absorption in the visible and NIR region, ranging from 753.6 to 2150 nm, which is higher than the surface (244 nm). Thus, these complexes have a potential for high-performance NLO materials in the applications of optics. Natural bond orbital analysis (NBO), transition density matrix (TDM), electron density difference map (EDDM), and density of state (DOS) analyses were also performed to study the charge transfer properties. Moreover, these complexes possessed remarkable optoelectronic properties due to a significant increase in the isotropic linear polarizability (α iso) in the range of 629.59-1423.23 au. Further, these systems demonstrated an extraordinary large total first hyperpolarizability (β tl) in the range of 3695.55-910 706.43 au. The rationalization of hyperpolarizability by the two-level model reflected a noteworthy increase in β tl because of low transition energies (ΔE) and high transition dipole moment (Δμ). Thus, our results showed that alkali and alkaline earth metal-doped BC might be a competitor for efficient nonlinear optical properties with practical applications in the area of optoelectronics.

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Metal-to-insulator crossover in alkali doped zeolite.

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